Abstract: Electrosorption technology has garnered extensive attention in the field of hexavalent uranium (U(Ⅵ)) recovery, attributed to its inherent advantages of low energy consumption, environmental benignity, and facile regeneration. However, critical technical bottlenecks, including insufficient active sites of electrode materials, inferior surface wettability, and the intrinsic ion exclusion effect, have severely restricted its large-scale practical application. To address these challenges, this study selected Gaultheria yunnanensis as the carbon precursor, which was subjected to activation and pore-forming processes to prepare nitrogen (N) and phosphorus (P) co-doped graphitized carbon. The resulting material was further fabricated into a monolithic electrode (denoted as NPC). On this basis, the doping nitrogen source was systematically optimized to enhance the active site density and electron transfer efficiency. Subsequently, the optimized NPC material was compounded with molybdenum disulfide (MoS₂) to construct a composite electrode (denoted as NPC/Mo), leveraging the synergistic effects between the two components. Material characterization and performance tests confirm that the NPC/Mo composite electrode possesses a stable three-dimensional (3D) porous network structure, which not only facilitates rapid mass transfer of U(Ⅵ) ions but also provides abundant channels for electrolyte penetration. Meanwhile, the electrode exhibits high specific capacitance and excellent U(Ⅵ) adsorption capacity, superior to the pristine NPC electrode. Systematic batch electrosorption experiments were conducted to investigate the effects of key operational parameters, revealing that the electrosorption behavior of U(Ⅵ) on both NPC and NPC/Mo electrodes is synergistically regulated by the applied voltage and solution pH. The applied voltage modulates the electric field intensity at the electrode-electrolyte interface, thereby affecting the electrostatic attraction between the electrode surface and U(Ⅵ) ions (predominantly existing as \mathrmUO_2^2+ in acidic conditions), while the solution pH influences the protonation state of functional groups on the electrode surface and the chemical speciation of U(Ⅵ), further regulating the adsorption mechanism. Kinetic analysis demonstrates that the U(Ⅵ) electrosorption process on both electrodes follows the pseudo-first-order kinetic model, indicating that the adsorption rate is dominated by physical adsorption and electrostatic attraction. Adsorption isotherm fitting results show that the process conforms to the Langmuir model, suggesting a monolayer adsorption mechanism on the homogeneous electrode surface. Under optimized operational conditions (applied voltage: 0.9 V; solution pH: 4.5), the maximum theoretical electrosorption capacity of the NPC/Mo electrode for U(Ⅵ) in low-concentration uranium solutions (initial concentration ≤50 ppm) reaches 109.01 mg/g, which is significantly higher than that of most reported carbon-based electrosorption electrodes. Systematic electrochemical tests, including cyclic voltammetry (CV) and galvanostatic charge-discharge measurements, indicates that the specific capacitance of the NPC/Mo electrode is 176.18 F/g, reflecting its excellent electrochemical storage capacity and charge transfer efficiency. Further mechanism studies reveal that the outstanding U(Ⅵ) electrosorption performance of the NPC/Mo electrode originates from the synergistic effect between electrical double-layer capacitance (EDLC) and pseudocapacitance. The 3D porous structure of the N, P co-doped graphitized carbon provides a large specific surface area for EDLC formation, while the redox reactions between MoS₂ and U(Ⅵ) contribute to pseudocapacitance, thereby enhancing the overall adsorption capacity. Additionally, the introduction of N and P doping and MoS₂ modification results in abundant functional groups (-NH-, -NH⁺-, and -OH) on the electrode surface, which not only serve as additional active sites for U(Ⅵ) chelation but also improve the surface wettability of the electrode. The mutual interactions and synergistic effects among these functional groups further strengthen the affinity between the electrode and U(Ⅵ) ions, significantly promoting the electrosorption efficiency. This study not only develops a high-performance composite electrode for U(Ⅵ) recovery but also provides a novel strategy for the design and fabrication of biomass-derived carbon-based composite materials, offering a promising solution for the efficient removal of U(Ⅵ) from low-concentration uranium-containing wastewater in nuclear industry and environmental remediation scenarios.